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Boreskov Institute of Catalysis of the Siberian Branch of Russian ...

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PP-IV-11OXIDATIVE CONVERSION OF METHANE AND METHANOL ONSTRUCTURED CATALYSTS M/Al 2 O 3 /CORDIERITE (M=Ni, Cu, Zn)S.A. Soloviev, A.Yu. Kapran, S.N. OrlykL.V. Pysarzhevskii <strong>Institute</strong> <strong>of</strong> Physical Chemistry <strong>of</strong> NAS, 31 Pr. Nauky,03028 Kyiv, Ukraine, fax: (044) 525 65 90, E-mail: orlyk@inphyschem-nas.kiev.uaAmong strategic problems <strong>of</strong> ХХІ century at transition from fundamental science toindustrial technologies <strong>the</strong> processes <strong>of</strong> steam and CO 2 conversion as well as partial oxidation<strong>of</strong> methane to carbon monoxide and hydrogen take leading positions [1]. In context <strong>of</strong>hydrogen fuel production reactions <strong>of</strong> methanol reforming are also in focus [2]. In this work<strong>the</strong> results <strong>of</strong> CO 2 conversion <strong>of</strong> methane and partial oxidation <strong>of</strong> methanol over structuredcatalysts – Ni/Al 2 O 3 - and Cu-ZnO/Al 2 O 3 - composites, applied on ceramic monoliths <strong>of</strong>honeycomb structure from syn<strong>the</strong>tic cordierite 2Al 2 O 3 ⋅2MgO⋅5SiO 2 (c), are presented. Thestructured alumo-nickel catalysts are shown to surpass essentially <strong>the</strong> conventional granulatedones with respect to productivity (CH 4 5.5, CO 2 7.0 % vol., 6000 h –1 ):CatalystTemperature <strong>of</strong> 80 %Productivity × 10 6CH 4 Conversion, °С Mol s –1 g –1 (cat.) Mol s –1 g –1 (NiO)GIAP-18, d=1-2 мм 485 12.96 1.628.2%NiO+11.2%Al 2 O 3 /c 480 38.3 4.83.8 % NiO/11.2%Al 2 O 3 /c 492 30.0 7.81.0 % NiO/2.0 % Al 2 O 3 /c 533 27.6 27.6The increase in stability <strong>of</strong> <strong>the</strong>ir work is achieved by regulation <strong>of</strong> <strong>the</strong> acid-baseproperties <strong>of</strong> a surface via introduction <strong>of</strong> alkali metal (Na, K) oxides. Such an approachcauses retardation <strong>of</strong> carbonization <strong>of</strong> <strong>the</strong> surface [3].In partial oxidation <strong>of</strong> methanol under stoichiometric conditions (С СН3ОН /С О2 = 4/2) onCu-ZnO/Al 2 O 3 /cordierite catalysts <strong>the</strong> yield <strong>of</strong> hydrogen is close to 90 %. A synergetic effectconsisting in decrease in selectivity <strong>of</strong> CO formation on Cu-ZnO-based catalyst, as comparedwith corresponding samples containing individual components Cu and ZnO, is found:Cu(ZnO) Percentage, CH 3 ОН Conversion, Selectivity, % Yield, %% wt.% /Т, °С Н 2 СО H 28 % Cu 79/505 23 26 188.5 % Cu, 7.5 % ZnO →100/505 88 5 886 % ZnO →100/495 89 13 89References1. Lonsford J.H., Catal.Today, 63 (2000) 165.2. Geissler K., Newson E., Vogel F. et al., Phys. Chem. Chem. Phys., 3 (2001) 289.3. Soloviev S.A., Kapran A.Yu., Orlyk S.N., Theor. and Experim. Chem., 43 (2007) 299.416

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